Polarized Raman scattering and magnetic ordering in Mn lightly doped van der Waals Cr1−xMnxGeTe3 crystals

A layered van der Waals ferromagnet CrGeTe3 has attracted considerable interest due to the great potential for exploring low-power functional spintronic devices. However, research on the incorporation of chemical substitution in CrGeTe3 to tune the lattice vibrations and magnetic interactions is still lacking. In this work, an understanding of the phonon property and magnetic orders in Mn lightly doped Cr1−xMnxGeTe3 single crystals has been reported. It is found that the phonon symmetries are preserved over the studied Mn substitution content, as confirmed by angle-resolved polarized Raman spectroscopy and first-principles calculations. Furthermore, clear signatures of improved ferromagnetic Curie–Weiss temperature and magnetic moment are observed by detailed magnetic measurements. The higher magnetic moment of Mn ions, the variation of Mn–Te–Cr angle, Mn-induced hole doping, and the concomitant strain effect may all contribute to the enhanced ferromagnetism. Overall, our results demonstrate that chemical substitution is an effective pathway to engineering the lattice and magnetism of CrGeTe3.